Ultrafast synthesis and binder‐free fabrication of a monolithic metal–organic framework for efficient carbon capture

Abstract Achieving rapid synthesis alongside efficient shaping without sacrificing high porosity and crystallinity poses significant challenges for metal–organic frameworks (MOFs) in practical applications. Here, we report an ultrafast, scalable method for preparing an ultramicroporous MOF at room temperature. This method achieves a space–time yield significantly higher than conventional MOF synthesis by orders of magnitude. As a result of strongly promoted crystal nucleation by careful selection of solvent and metal source, the MOF material is produced in a gel state offering both high crystallinity and processability. This allows for the binder‐free fabrication of monolithic adsorbents with predesigned macro shapes and sizes. Owing to its narrowly distributed pore size and high‐density open metal sites, the monolithic adsorbent demonstrates top‐tier selectivity for CO 2 /N 2 (>200) and CO 2 /CH 4 separations. The performance sets a new benchmark among current MOF xero‐ or aerogel monoliths. Breakthrough experiments further verify its robust ability for carbon capture under dynamic conditions.